Crystallization tailoring of cesium/formamidinium double-cation perovskite for efficient and highly stable solar cells

Abstract Achieving high-quality perovskite crystal films is a critical prerequisite in boosting solar cell efficiency and improving the device stability, but the delicate control of nucleation and growth of the perovskite film remains limited success. Herein, a facile but effective strategy has been developed to finely tailor the crystallization of thermally stable cesium/formamidinium (Cs/FA) based perovskite via partially replacing PbI2 with PbCl2 in the precursor solution. The incorporation of chlorine into the perovskite crystal lattice derived from PbCl2 changes the crystallization process and improves the crystal quality, which further results in the formation of larger crystal grains compared to the control sample. The larger crystal grains with high crystallinity lead to reduced grain boundaries, suppressed non-radiative recombination, and enhanced photoluminescence lifetime. Under the optimized conditions, the methylammonium free perovskite solar cells (PSCs) delivers a champion power conversion efficiency (PCE) of 21.30% with an open-circuit voltage as high as 1.18 V, which is one of the highest efficiencies for Cs/FA based PSCs up to now. Importantly, the unencapsulated PSC devices retain more than 95% and 81% of their original PCEs even after long-term (over one year) storage under ambient conditions or 2000 h's thermal aging at 85 °C in a nitrogen atmosphere, respectively.